Coordination-assembly synthesis of Pt-based high-entropy oxide catalysts for VOC oxidation: dual role of ligands in reducing formation barrier and anchoring active sites
文献类型: 外文期刊
作者: Xiao Zhang;Wenxin Liu;Feng Shen;Boxiong Shen;Shuhao Li
作者机构:
关键词: Catalytic oxidation;Coordination-assembly;High entropy oxide;Pt dispersion;Volatile organic compounds
期刊名称: Separation and Purification Technology
ISSN: 1383-5866
年卷期: 2026 年 389 卷
页码:
收录情况: SCIE(2025版) ; ; EI(2025版)
摘要: The development of high-entropy oxide (HEO) catalysts is often limited by high synthesis temperatures and low surface areas, which restrict their effectiveness in volatile organic compound (VOC) oxidation. In this study, we propose a novel coordination-assembly method for synthesizing Pt-based HEO catalysts, where organic ligands serve dual functions: (i) reducing the formation energy barrier for HEO crystallization and (ii) anchoring Pt precursors during synthesis. This dual effect enables the formation of spinel-phase HEO (HEO-C) at a relatively low synthesis temperature (600 °C), with a significantly enhanced BET surface area of 22.8 m2/g, markedly higher than that of conventionally synthesized HEOs (<5 m2/g). The resulting Pt@HEO-C catalyst exhibits excellent catalytic performance for o-xylene oxidation, achieving a T90 at 231 °C, significantly lower than those of Pt catalysts supported on conventional HEOs and mixed oxides. In-situ DRIFTS and GC–MS analyses confirm that the Pt@HEO-C catalyst facilitates the further oxidation of ring-opening intermediates, improving reaction selectivity. Density functional theory calculations reveal enhanced Pt dispersion, uniform adsorption energetics, and stronger Pt-support charge transfer in the Pt@HEO-C catalyst. The catalyst also shows remarkable sulphur tolerance and long-term stability. This work demonstrates the potential of ligand-directed coordination-assembly strategies in constructing high-surface-area HEOs at low temperatures for advanced VOC oxidation applications.
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